Process of producing motor fuels by destructive hydrogenation of carbonaceous material



Patented June 21, 1932 UNITED STATES PATENT orgiba MATHIAS PIER, OF HEIDELIBERG, AND MARTIN MIlLLER-CUNRADI, OE LUDWIGSHAFEN- ON-THE-RHINE, GERMANY, ASSIGNORS TO I. G. FARBENINDUSTRIE AKTIENGESELL- SCHAFT, OF FRANKFORT-ON-THE-MAIN, GERMANY, A CORPORATION OF GERMANY PROCESS OF PRODUCING MOTOR FUELS BY DESTRUCTIVE HYDROGENATION OF OARBONACEOUS MATERIAL No Drawing. Application filed November 14, 1927, Serial No. 233,312, and in Germany November 26, 1926.

By the destructive hydrogenation of solid.

non-asphaltic carbonaceous materials such as various kinds of pyrobituminous materials such as coal, especially brown-coal containing a high content of bitumen, motor fuels, especially hydrocarbons of low boiling point, such asbenzine, are obtained which are very liable to knock.

We have now found that knocking of the said motor fuels is due to the presence of liquid hydrocarbon products of low boillng point formed by the destructive hydrogenation of the bitumen of the coal and the primary conversion products of the former such as parafiin wax and that excellent motor fuels, which are not inclined to knocking, are obtained from bituminous, and even highly bituminous kinds of coal, especially brown-coal when working under such conditions that the bitumen itself or its primary conversion products such as parafiin wax are not converted, or only to a slight extent, into low-boiling products, especially benzine, whereas the other constituents of the coal are converted to a large extent into such products. The term bitumen is intended to include for the purposes of the present invention all those constituents which can be extracted from the coal by means of a solvent of the nature of benzene and its equivalents. The process according to the present invention may be carried out in various ways.

An advantageous method of procedure is to eliminate the bitumen, which expression is also intended to include its primary conversion products, prior to, or during any intermediate stage in, the treatment of the bituminous material.

The bitumen may be removed in any convenient manner, for example by extracting the raw material with benzene or similar solvents at atmospheric or elevated pressure. The resulting coal, free from or low in bitumen is then treated with hydrogen at elevated pressure and temperature, with or without catalysts and, under these conditions, a satisfactory non-knocking motor fuel is obtained.

The removal of the bitumen or its primary conversion products such as paraflin waxes, may also be effected in an intermediate stage of the treatment by separation, for example by cooling to low temperatures, from the rather heavy oils of approximately middle-oil character, that is to say such boiling mainly between about 200 and 325 C. obtained in the first stage of the process.

According to this manner of working, the A heavy oils of approximately middle oil char-' acter are obtained without a substantial conversion of the, bitumen by treating the pyrobituminous material under the mildest of the conditions of destructive hydrogenation capable of producing liquefaction of the pyrobituminous material in a reasonable Example 1 Brown-coal, containing 8 to 10 per cent of bitumen and furnishing, on' treatment with hydrogen at an elevated temperature of about 425 C. and under a pressure of about 200 atmospheres in the presence of a, catalyst prepared from molybdic acid and'zinc oxide, a

benzinc exhibiting a tendency to knock in an internal combustion engine with the ratio of compression, that is to say the ratio between the volume of the cylinder at the end of the compression stroke and the volume 0! the cylinder at the beginning of the compression stroke 1:5, is freed wholly or for the most part from bitumen by extraction with benzene. The benzine then obtained by destructive hydrogenation under the same conditions does not knock under the same conditions of compression.

Instead of removing the bitumen prior to the hydrogen treatment, the products obtained from the bitumen during the treat ment of the coal with hydrogen by stages can be removed in any intermediate stage.

For example, the coal maybe extensively converted into middle oils which are cooled I to a low temperature, say to about 40 to 60 C. below zero, so that the bitumen or paraffin wax can be removedin the solid f orm and the productthus fiedfrom bitumen is then converted into benzine. What weclaim is:

1. ,A process for the production of motor 1 fuels not inclined to knocking from a solid non-asphalticpyrobituminous material having a high bitumen content which comprises removing substantially only the biturnen from said material and thereupon subj ectingthe resulting residue to destructive hydrogenation. v

2. A process for the production of motor fuels not inclined toknocking from a solid non-asphaltic pyrobituminous material having a hi h bitumen content which comprises e'x racting the bitumen from said materialwith the aid of a solvent of the naw' ture of benzene and thereupon subjecting the resulting residue to destructive hydrogenation. A

3. A process for the production of motor fuels not inclined to knocking from a solid non-asphaltic' pyrobitumi'nous' material having a high,bitumen content which comprises extracting-the bitumen from said material with theaid of a benzene hydrocarbon and thereupon subjecting the resulting residue to destructive hydrogenation.

4. In the process for producing non-knocking motor fuels by destructive hydrogenation ofsolid non-asphaltic pyrobitu'minous ma- 0 teri'als having a high bitumen content under'pressure, the steps of effecting removal of the'bitumens in a substantially unconyertedfstate prior to'the completion of the hydrogenation and completing the h dro- *5 genation of the bitumen free materia 5."'The process for the production of nonknocking -motor fuels from solid nonasphaltic pyrobituminous materials hav-' ing a high bitumen content which comprises extracting the bitumens from said materials 'by a" treatment with ben-.

ze ne under an elevated temperature and pressure and-"subjecting the residual materials to destructive hydrogenation. 1'

, 6. The process as defined in claim 5 wherein the solid [non-asphaltic pyrobituminous' material is brown coal.

In testimony whereof we have hereunto set our hands. 7 n MATHIAS PIER.

MARTIN MULLER-CUNBADI; 

